通过氢化物介导的区域选择性掺杂到（Pd@Au）中来合成三金属（HPd@MAu）超原子（M = Ag，Cu）。
Synthesis of Trimetallic (HPd@MAu) Superatoms (M = Ag, Cu) via Hydride-Mediated Regioselective Doping to (Pd@Au).
作者信息
Hirai Haru, Takano Shinjiro, Tsukuda Tatsuya
机构信息
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.
Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Katsura, Kyoto 615-8520, Japan.
出版信息
ACS Omega. 2019 Apr 18;4(4):7070-7075. doi: 10.1021/acsomega.9b00575. eCollection 2019 Apr 30.
We have recently reported that hydride (H) doped superatom (HPd@Au) protected by eight PPh ligands selectively grew into (HPd@Au) by the nucleophilic addition of two Au(I)Cl units. In the present study, (HPd@Au) was successfully converted to unprecedented trimetallic (HPd@MAu) superatoms (M = Ag, Cu) by controlled doping of two Ag(I)Cl or Cu(I)Cl units, respectively. Single-crystal X-ray diffraction analysis demonstrated that two Ag(I) or Cu(I) ions were regioselectively incorporated. Theoretical calculations suggested that hydrogens in (HPd@MAu) (M = Au, Ag, Cu) occupy the same bridging site between the central Pd atom and the surface Au atom. (HPd@AgAu) exhibited photoluminescence at 775 nm, with the enhanced quantum yield of 0.09%, although it is structurally and electronically equivalent with (HPd@Au). This study demonstrates that hydride-mediated growth process is a promising atomically-precise bottom-up synthetic method of new multimetallic superatoms.
我们最近报道，由八个三苯基膦（PPh）配体保护的氢化物（H）掺杂超原子（HPd@Au）通过两个Au(I)Cl单元的亲核加成选择性地生长为（HPd@Au）。在本研究中，通过分别控制掺杂两个Ag(I)Cl或Cu(I)Cl单元，（HPd@Au）成功转化为前所未有的三金属（HPd@MAu）超原子（M = Ag，Cu）。单晶X射线衍射分析表明，两个Ag(I)或Cu(I)离子被区域选择性地掺入。理论计算表明，（HPd@MAu）（M = Au，Ag，Cu）中的氢占据中心Pd原子和表面Au原子之间的相同桥连位点。（HPd@AgAu）在775 nm处表现出光致发光，量子产率提高了0.09%，尽管它在结构和电子性质上与（HPd@Au）相当。这项研究表明，氢化物介导的生长过程是一种有前途的、原子精确的自下而上合成新型多金属超原子的方法。
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